Publications

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Simplified models that are based on macroscopic force balances and droplet-geometry approximations are presented for predicting the onset of instability leading to removal of water droplets at the gas diffusion layer (GDL)/gas flow channel (GFC) interface. Visualization experiments are carried out to observe the formation, growth, and removal or instability of the water droplets at the GDL/GFC interface of a simulated polymer electrolyte fuel cell cathode. Droplet-instability diagrams or windows computed by the simplified models are compared with those measured experimentally, and good agreement is obtained. Two-dimensional flow simulations employing the finite element method coupled with an arbitrary Lagrangian-Eulerian formulation for determining the liquid/gas interface position are also performed to assess the simplified cylindrical-droplet model. Necessary conditions for preventing fully grown droplets from lodging in the flow channel are derived using the simplified models. It is found that droplet removal can be enhanced by increasing flow channel length or mean gas flow velocity, decreasing channel height or contact angle hysteresis, or making the GDL/GFC interface more hydrophobic.

This report documents the author's efforts in the deterministic modeling of copper-sulfidation corrosion on non-planar substrates such as diodes and electrical connectors. A new framework based on Goma was developed for multi-dimensional modeling of atmospheric copper-sulfidation corrosion on non-planar substrates. In this framework, the moving sulfidation front is explicitly tracked by treating the finite-element mesh as a pseudo solid with an arbitrary Lagrangian-Eulerian formulation and repeatedly performing re-meshing using CUBIT and re-mapping using MAPVAR. Three one-dimensional studies were performed for verifying the framework in asymptotic regimes. Limited model validation was also carried out by comparing computed copper-sulfide thickness with experimental data. The framework was first demonstrated in modeling one-dimensional copper sulfidation with charge separation. It was found that both the thickness of the space-charge layers and the electrical potential at the sulfidation surface decrease rapidly as the Cu{sub 2}S layer thickens initially but eventually reach equilibrium values as Cu{sub 2}S layer becomes sufficiently thick; it was also found that electroneutrality is a reasonable approximation and that the electro-migration flux may be estimated by using the equilibrium potential difference between the sulfidation and annihilation surfaces when the Cu{sub 2}S layer is sufficiently thick. The framework was then employed to model copper sulfidation in the solid-state-diffusion controlled regime (i.e. stage II sulfidation) on a prototypical diode until a continuous Cu{sub 2}S film was formed on the diode surface. The framework was also applied to model copper sulfidation on an intermittent electrical contact between a gold-plated copper pin and gold-plated copper pad; the presence of Cu{sub 2}S was found to raise the effective electrical resistance drastically. Lastly, future research needs in modeling atmospheric copper sulfidation are discussed.

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This report documents the efforts and accomplishments of the LIGA electrodeposition modeling project which was headed by the ASCI Materials and Physics Modeling Program. A multi-dimensional framework based on GOMA was developed for modeling time-dependent diffusion and migration of multiple charged species in a dilute electrolyte solution with reduction electro-chemical reactions on moving deposition surfaces. By combining the species mass conservation equations with the electroneutrality constraint, a Poisson equation that explicitly describes the electrolyte potential was derived. The set of coupled, nonlinear equations governing species transport, electric potential, velocity, hydrodynamic pressure, and mesh motion were solved in GOMA, using the finite-element method and a fully-coupled implicit solution scheme via Newton's method. By treating the finite-element mesh as a pseudo solid with an arbitrary Lagrangian-Eulerian formulation and by repeatedly performing re-meshing with CUBIT and re-mapping with MAPVAR, the moving deposition surfaces were tracked explicitly from start of deposition until the trenches were filled with metal, thus enabling the computation of local current densities that potentially influence the microstructure and frictional/mechanical properties of the deposit. The multi-dimensional, multi-species, transient computational framework was demonstrated in case studies of two-dimensional nickel electrodeposition in single and multiple trenches, without and with bath stirring or forced flow. Effects of buoyancy-induced convection on deposition were also investigated. To further illustrate its utility, the framework was employed to simulate deposition in microscreen-based LIGA molds. Lastly, future needs for modeling LIGA electrodeposition are discussed.

The process of removing liquid water droplets in polymer electrolyte fuel cells (PEFC) is examined using a simple analytical model and two-dimensional simulations. Specifically, the stability of a droplet adhering to the wall of the cathode flow channel is examined as a function of the geometry of the flow channel, the applied pressure gradient, and the wetting properties. The result is a prediction of the critical droplet size as a function of the difference between the advancing and receding contact angles, or contact angle hysteresis. The analytical model is shown to qualitatively predict this stability limit when compared to two-dimensional simulation results. The simulations are performed using both Arbitrary Lagrangian Eulerian (ALE) methods and level set methods. The ALE and level set predictions are shown to be in good agreement. Copyright © 2004 by ASME.

Two-dimensional processes of nickel electrodeposition in LIGA microfabrication were modeled using the finite-element method and a fully coupled implicit solution scheme via Newtons technique. Species concentrations, electrolyte potential, flow field, and positions of the moving deposition surfaces were computed by solving the species-mass, charge, and momentum conservation equations as well as pseudo-solid mesh-motion equations that employ an arbitrary Lagrangian-Eulerian (ALE) formulation. Coupling this ALE approach with repeated re-meshing and re-mapping makes it possible to track the entire transient deposition processes from start of deposition until the trenches are filled, thus enabling the computation of local current densities that influence the microstructure and functional/mechanical properties of the deposit.

Electrodeposition is a key process in LIGA (Lithographie, Galvanoformung, Abformung - German words for lithography, electroplating and molding) - microfabrication, which is increasingly demonstrated to be a viable technology for fabricating micro-devices or parts. LIGA Electrodeposition involves complex multi-physics phenomena: (1) diffusion, migration, and convection of charged species in a centimeter-scale electrolyte-bath region and in micron-scale featurecavity or trench regions; (2) homogeneous and heterogeneous electrochemical reactions; and (3) moving deposition surface or surfaces on which metal ions (e.g., {approx} i) are electrochemically reduced to form a pure metal or an alloy.

An analytical capability is being developed that can be used to predict the effect of corrosion on the performance of electrical circuits and systems. The availability of this ''toolset'' will dramatically improve our ability to influence device and circuit design, address and remediate field occurrences, and determine real limits for circuit service life. In pursuit of this objective, we have defined and adopted an iterative, statistical-based, top-down approach that will permit very formidable and real obstacles related to both the development and use of the toolset to be resolved as effectively as possible. An important component of this approach is the direct incorporation of expert opinion. Some of the complicating factors to be addressed involve the code/model complexity, the existence of large number of possible degradation processes, and an incompatibility between the length scales associated with device dimensions and the corrosion processes. Two of the key aspects of the desired predictive toolset are (1) a direct linkage of an electrical-system performance model with mechanistic-based, deterministic corrosion models, and (2) the explicit incorporation of a computational framework to quantify the effects of non-deterministic parameters (uncertainty). The selected approach and key elements of the toolset are first described in this paper. These descriptions are followed by some examples of how this toolset development process is being implemented.

A transient, multidimensional model has been developed to simulate proton exchange membrane fuel cells. The model accounts simultaneously for electrochemical kinetics, current distribution, hydrodynamics, and multicomponent transport. A single set of conservation equations valid for flow channels, gas-diffusion electrodes, catalyst layers, and the membrane region are developed and numerically solved using a finite-volume-based computational fluid dynamics technique. The numerical model is validated against published experimental data with good agreement. Subsequently, the model is applied to explore hydrogen dilution effects in the anode feed. The predicted polarization curves under hydrogen dilution conditions are in qualitative agreement with recent experiments reported in the literature. The detailed two-dimensional electrochemical and flow/transport simulations further reveal that in the presence of hydrogen dilution in the fuel stream, hydrogen is depleted at the reaction surface, resulting in substantial anode mass transport polarization and hence a lower current density that is limited by hydrogen transport from the fuel stream to the reaction site. Finally, a transient simulation of the cell current density response to a step change in cell voltage is reported.

Two-phase flow and transport of reactants and products in the air cathode of proton exchange membrane (PEM) fuel cells is studied analytically and numerically. Four regimes of water distribution and transport are classified by defining three threshold current densities and a maximum current density. They correspond to first appearance of liquid water at the membrane/cathode interface, extension of the gas-liquid two-phase zone to the cathode/channel interface, saturated moist air exiting the gas channel, and complete consumption of oxygen by the electrochemical reaction. When the cell operates above the first threshold current density, liquid water appears and a two-phase zone forms within the porous cathode. A two-phase, multi-component mixture model in conjunction with a finite-volume-based computational fluid dynamics (CFD) technique is applied to simulate the cathode operation in this regime. The model is able to handle the situation where a single-phase region co-exists with a two-phase zone in the air cathode. For the first time, the polarization curve as well as water and oxygen concentration distributions encompassing both single- and two-phase regimes of the air cathode are presented. Capillary action is found to be the dominant mechanism for water transport inside the two-phase zone. The liquid water saturation within the cathode is predicted to reach 6.3% at 1.4 A/cm{sup 2}.

A phenomenological model was developed for multicomponent transport of charged species with simultaneous electrochemical reactions in concentrated solutions, and was applied to model processes in a thermal battery cell. A new general framework was formulated and implemented in GOMA (a multidimensional, multiphysics, finite-element computer code developed and being enhanced at Sandia) for modeling multidimensional, multicomponent transport of neutral and charged species in concentrated solutions. The new framework utilizes the Stefan-Maxwell equations that describe multicomponent diffusion of interacting species using composition-insensitive binary diffusion coefficients. The new GOMA capability for modeling multicomponent transport of neutral species was verified and validated using the model problem of ternary gaseous diffusion in a Stefan tube. The new GOMA-based thermal battery computer model was verified using an idealized battery cell in which concentration gradients are absent; the full model was verified by comparing with that of Bernardi and Newman (1987) and validated using limited thermal battery discharge-performance data from the open literature (Dunning 1981) and from Sandia (Guidotti 1996). Moreover, a new Liquid Chemkin Software Package was developed, which allows the user to handle manly aspects of liquid-phase kinetics, thermodynamics, and transport (particularly in terms of computing properties). Lastly, a Lattice-Boltzmann-based capability was developed for modeling pore- or micro-scale phenomena involving convection, diffusion, and simplified chemistry; this capability was demonstrated by modeling phenomena in the cathode region of a thermal battery cell.

A low-cost, thermally-activated, palladium-catalyzed metallization process was developed for rapid prototyping of polymeric electronic substrates and devices. The process was successfully applied in producing adhesiveless copper/polyimide laminates with high peel strengths and thick copper coating; copper/polyimide laminates are widely used in fabricating interconnects such as printed wiring boards (PWBs) and flexible circuits. Also successfully metallized using this low-cost metallization process were: (1) scaled-down models of radar-and-communication antenna and waveguide; (2) scaled-down model of pulsed-power-accelerator electrode; (3) three-dimensional micro-porous, open-cell vitreous carbon foams. Moreover, additive patterned metallization was successfully achieved by selectively printing or plotting the catalyst ink only on areas where metallization is desired, and by uniform thermal activation. Additive patterned metallization eliminates the time-consuming, costly and environmentally-unfriendly etching process that is routinely carried out in conventional subtractive patterned metallization. A metallization process via ultraviolet (UV) irradiation activation was also demonstrated. In this process palladium-catalyst solution is first uniformly coated onto the substrate. A masking pattern is used to cover the areas where metallization is not wanted. UV irradiation is applied uniformly to activate the palladium catalyst and to cure the polymer carrier in areas that are not covered by the mask. Metal is then deposited by electroless plating only or by a combination of electroless and electrolytic plating. This UV-activation technique is particularly useful in additive fine-line patterned metallization. Lastly, computer models for electrolytic and electroless plating processes were developed to provide guidance in plating-process design.

Highly porous sol-gel films have potential applications as electrical and thermal insulators, catalyst supports, sensors, and membranes for gas separations. Pore dimensions in these sol-gel films are usually small e.g., on the order of tens of nanometers or less. Their successful fabrications, however, greatly depend on the fundamental understanding of mechanisms that underlie the phenomena of pore evolution, network shrinkage, and stress development since the final microstructure of a solid gel film is strongly affected by composition of its starting sol and its processing conditions. This report documents a simplified one-dimensional analysis of drying a solidifying sol-gel thin film coating supported by an impermeable solid substrate. Portions of this work were presented at the 1994 Annual Joint Meeting of the New Mexico Section of the American Ceramic Society and Materials Research Society in Albuquerque. The authors considered the solid/liquid two phase coexistent regime during the drying solidifying process in which solvent is removed continuously via evaporation, the solid phase grows significantly in mechanical strength, and pore space shrinks appreciably. From overall and differential mass balances and a force balance at equilibrium, coupled with empirical correlations of solid phase modulus and permeability to strain or deformation, the authors followed the evolution of pore space, solid phase elastic stress, and liquid phase hydrodynamic pressure; they also determined their respective values at equilibrium. By assuming microscopic pore shape models, they estimated and compared the predicted mean pore radii. Their simplified one-dimensional analysis shows that the final mean pore radius is controlled by four parameters: pore-liquid surface tension, solid phase modulus, mean pore radius, and porosity at the initial stress-free state. The one-dimensional model can be employed to guide process design and optimization in sol-gel film fabrications.

Electroless deposition of copper is being used for a variety of applications, one of them being the development of seed metallic layers on non-metals, which are widely used in electronic circuitry. Solution equilibrium characteristics of two electroless copper baths containing EDTA and tartrate as the complexing agents were studied as functions of pH, chelating agent and metal ion concentrations. Equilibrium diagrams were constructed for both cu-tartrate and Cu-EDTA systems. It was determined that copper is chiefly complexed as Cu(OH){sub 2}L{sub 2}{sup {minus}4} in the tartrate bath, and as CuA{sup {minus}2} in the EDTA bath, where L and A are the complexing tartrate and EDTA ligands, respectively. The operating ranges for electroless copper deposition were identified for both baths. Dependence of Cu(OH){sub 2} precipitation on the pH and species concentrations was also studied for these systems.

Slide coating flow is a workhorse process for manufacturing precision film-coating products. Properly starting up a slide coating process is very important in reducing wastage during startup and ensuring that the process operates within the desired `coating window.` A two-phase flow analysis of slide-coating startup was performed by Palmquist and Scriven (1994) using Galerkin`s method with finite-element basis functions and an elliptic mesh generation scheme. As reported by Chen (1992) from flow visualization experiments, a continuously coated liquid film breaks up into rivulets, which are coating stripes with dry lanes in between, when the coated film becomes thinner and thinner due to either the increase in substrate speed or the reduction in pre-metered feed-liquid pump speed. It was observed that the coated-film breakup process originated from the coating bead, thus the name of bead breakup. Understanding the bead-breakup phenomena and elucidating mechanisms involved will provide guidance for manufacturing thinner coating, an industrial trend for better product performance. In this paper we present simulation results of slide-coating flows obtained from a computational method capable of describing arbitrary, three-dimensional and time-dependent deformations. The method, which is available in a commercial code, uses a fixed grid through which fluid interfaces are tracked by a Volume-of-Fluid technique (Hirt and Nichols, 1981). Surface tension, wall adhesion, and viscous stresses are fully accounted for in our analysis. We illustrate our computational approach by application to startup and the bead-breakup problems. As will be shown, for rapid processes our approach offers the computational efficiency and robustness that are difficult o achieve in conventional finite-element-based methods.

In coating processes (e.g. in blade coating) the flow domain inherently contains free surfaces and three-phase contact lines, and characteristic length scales of flow features in the dimension transverse to the web-movement vary by an order of magnitude or more from a fraction of a millimeter or more to tens of microns or less). The presence of free surfaces and three-phase contact lines, and the sudden changes of flow geometry and directions create difficulties in theoretical analyses of such flows. Though simulations of coating flows via finite-element methods using structured grids have been reportedly demonstrated in the literature, achieving high efficiency of such numerical experiments remains a grand challenge -- mainly due to difficulties in local mesh-refinement and in avoiding unacceptably distorted grids. High efficiency of computing steady flow fields under various process conditions is crucial in shortening turn-around time in design and optimization of coating-flow processes. In this paper we employ a fully-implicit, pseudo-solid, domain mapping technique coupled with unstructured meshes to analyze blade and slot coating flows using Galerkin`s method with finite element basis functions. We demonstrate the robustness and efficiency of our unique technique in circumventing shortcomings of mesh-motion schemes currently being used in the coating-flow research community. Our goal is to develop an efficient numerical tool, together with a suitable optimization toolkit, that can be used routinely in design and optimization of coating-flow processes.

A brief history of lightning protection at Pantex nuclear explosive areas (NEAs) is given. An assessment of current Pantex lightning protection at NEAs is summarized. Recommendations for further improvements in lightning protection are described.

Translations of two pioneering Russian papers on antenna theory are presented. The first paper provides a treatise on finite-length dipole antennas; the second paper addresses infinite-length, impedance-loaded transmitting antennas.